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Study of Catalytic Oxidation of Cyclohexane over Supported Metalloporphyrin in Fixed-bed Reactor

Author: YangShuRen
Tutor: LiuZhiGangï¼›GuoCanCheng
School: Hunan University
Course: Organic Chemistry
Keywords: Metalloporphyrins Load Cyclohexane Selective oxidation Fixed-bed reactor
CLC: O643.32
Type: Master's thesis
Year: 2010
Downloads: 100
Quote: 3
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Abstract


The enzyme is a biological catalyst, it has good catalytic activity and selectivity specificity Therefore, in the situation of global warming, the research and development of biomimetic catalysts with enzymatic properties has important social value and significance. Metalloporphyrins studied a class of biomimetic catalysts currently used in the activation of the alkane oxidation reaction. However, in a homogeneous system, the metal porphyrin presence of auto-oxidation, dimer, and can not be recycled, but most of the tank reactor process is complex and difficult to control of reaction conditions. Therefore, the homogeneous catalyst multiphase, and applied to the fixed bed reaction system is not only conducive to overcome the problem of metal porphyrin catalyst stability is poor and can not be recycled, and the process is simple, continuous production. In this paper, the effects of carrier and preparation method on the catalytic activity of metalloporphyrins, also investigated the catalytic properties of different types of catalyst in the catalytic oxidation of cyclohexane in air, and then filter out the metal with the highest catalytic performance porphyrin catalyst and optimized reaction conditions, the last preliminary reaction mechanism was discussed. The main contents are as follows: 1. Were investigated small kettle sampling off-line detection and online real-time analysis and other detection methods, finally established chlorobenzene as the internal standard real-time online analysis methods. Preparation load metal porphyrins, oxides, and modified molecular sieve catalyst, investigated the impact of gas-phase oxidation reaction of cyclohexane, filter out the optimum catalytic performance of the catalyst, TPPCo/13X catalyst. The catalytic activity of various catalysts order: metal tetraphenyl porphyrin GT load; modified 13X molecular sieve GT; metal oxides. The ScS life of the catalyst. Continuous reaction 20 h under optimized conditions, the cyclohexane conversion rate fell from 18.2% to 16.1% alcohol and ketone, and cyclohexene selectivity little change in selectivity to alcohol and ketone is kept at about 3-4%, ring The hexene selective about 5% the pentanal selective process and then increased from the beginning of 1.4% to 0.6% and then rebounded to 1.1%. Catalyst for a long time to be able to maintain good stability. 4 examines the performance of the catalyst can be reused. Found in the end of the reaction at elevated temperatures and continuous ventilation 3h and then repeating the reaction under the reaction conditions, the catalyst having high activity. Repeat a third time when the conversion rate of cyclohexane, cyclohexene, cyclohexanol and cyclohexyl ketone product selectivity with the first compared with little change. 5 in conjunction with the experimental data and the phenomenon of the reaction process and oxidation products may be generated route.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalytic reaction
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